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DOE OSTI2024

Plutonium Speciation and Oxidation State Distributions in the Presence of Citrate

We explored the speciation and kinetics of the Pu(VI)-citrate and Pu(III)-citrate systems (pH m = 2.5–11.0, I = 0.1 M NaCl, T = 23 °C, O 2 (g) < 2 ppm) using ultraviolet–visible–near-infrared (UV–vis–NIR) spectrophotometry, solvent extraction, and PHREEQC modeling. Formation constants were determined for PuO 2 (HcitH)(aq) (log K° 1,1 = 1.09 ± 0.05) and PuO 2 (HcitH)(citH) 3– (log K° 1,2 = -0.20 ± 0.07), and evidence for (PuO 2 ) m (citH –k ) n (OH) x 2m(3+k)n–x was identified under alkaline conditions. Pu(VI) species were found to be less stable in the presence of citrate than in the absence of citrate (t ≤ 168 days); the rate of reduction increased with increasing pH. Further, the direct reduction of Pu(VI) to Pu(IV) was required to fit experimental data in the presence of citrate but did not improve the fit for Pu in the absence of citrate. We also observed increased Pu(III) stability in the presence of citrate (t ≤ 293 days), with higher concentrations of Pu(III) favored at lower pH. Finally, we provide evidence of a radiolysis-driven mechanism for the citrate-mediated reduction of plutonium that involves electron transfer from the oxidative breakdown of citrate. Our work highlights the need to investigate the redox effect of organic ligands on plutonium oxidation states under repository-relevant conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Pu-240 Target Preparation on Thin Backing Foils for GRETINA Experiments using ATLAS

Recent measurements of the octupole strength to the highest spin states in Pu-240 were performed using sub-barrier Coulomb excitation in order to unambiguously and convincingly demonstrate the existence of the rotational-aligned phonon condensation in this nucleus. The Pu-240 targets were prepared at the Center for Accelerator Target Science by molecular plating onto thin backing foils of C and Al. The required plutonium oxide dissolution, molecular plating methodology, plating results, and in-beam target performance will be discussed.

Actinides↗

DOE OSTI2014

Cross-correlation measurements with the EJ-299-33 plastic scintillator

New organic–plastic scintillation compositions have demonstrated pulse-shape discrimination (PSD) of neutrons and gamma rays. We present cross-correlation measurements of 252 Cf and mixed uranium–plutonium oxide (MOX) with the EJ-299-33 plastic scintillator. For comparison, equivalent measurements were performed with an EJ-309 liquid scintillator. Offline, digital PSD was applied to each detector. These measurements show that EJ-299-33 sacrifices a factor of 5 in neutron–neutron efficiency relative to EJ-309, but could still utilize the difference in neutron–neutron efficiency and neutron single-to-double ratio to distinguish 252 Cf from MOX. These measurements were modeled with MCNPX-PoliMi, and MPPost was used to convert the detailed collision history into simulated cross-correlation distributions. MCNPX-PoliMi predicted the measured 252 Cf cross-correlation distribution for EJ-309 to within 10%. Greater photon uncertainty in the MOX sample led to larger discrepancy in the simulated MOX cross-correlation distribution. In conclusion, the modeled EJ-299-33 plastic also gives reasonable agreement with measured cross-correlation distributions, although the MCNPX-PoliMi model appears to under-predict the neutron detection efficiency.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2016

A compact neutron scatter camera for field deployment

Here, we describe a very compact (0.9 m high, 0.4 m diameter, 40 kg) battery operable neutron scatter camera designed for field deployment. Unlike most other systems, the configuration of the sixteen liquid-scintillator detection cells are arranged to provide omnidirectional (4π) imaging with sensitivity comparable to a conventional two-plane system. Although designed primarily to operate as a neutron scatter camera for localizing energetic neutron sources, it also functions as a Compton camera for localizing gamma sources. In addition to describing the radionuclide source localization capabilities of this system, we demonstrate how it provides neutron spectra that can distinguish plutonium metal from plutonium oxide sources, in addition to the easier task of distinguishing AmBe from fission sources.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2015

Analysis of Powder Airborne Release Fractions for Vessel Ruptures

The Department of Energy handbook for airborne releases from nonreactor nuclear facilities bases its bounding airborne release fraction (ARF) for pressurized powders on tests conducted at Pacific Northwest Laboratory (PNL). An analysis is presented that correlates the ARF from these tests. The amount of powder that becomes airborne is correlated in terms of an adjusted airborne release fraction (AARF) equal to the product of the powder entrainment from the powder bed and the ratio of the total vessel volume to the volume occupied by the powder bed. Powder entrainments and release fractions at low pressures are correlated using a fluidized bed analogy. The analysis shows that the entrainment is enhanced by a sonic shock if the pressure prior to the rupture exceeds approximately 33 psig. A secondary, three-dimensional shock is predicted to occur at an initial pressure of approximately 332 psig. A correlation based on this analysis is used to predict the ARF for ruptures of vessels containing plutonium oxide. It is assumed that the oxide is pressurized by hydrogen that is radiolytically generated from adsorbed moisture.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2015

242 PU Standards Documentation Package

The standards documented in this package are composed of plutonium oxide. One set of standards was fabricated from 84% 242 pu material and the other 89% 242 pu material. They were specifically designed to be used as calibration standards for thermal neutron counters (TNCs). The procedure used to prepare these standards is part of the documentation package.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2016

FY 2016 Status Report: Documentation of All CIRFT Data including Hydride Reorientation Tests (Draft M2)

The first portion of this report provides a detailed description of fiscal year (FY) 2015 test result corrections and analysis updates based on FY 2016 updates to the Cyclic Integrated Reversible-Bending Fatigue Tester (CIRFT) program methodology, which is used to evaluate the vibration integrity of spent nuclear fuel (SNF) under normal conditions of transport (NCT). The CIRFT consists of a U-frame test setup and a real-time curvature measurement method. The three-component U-frame setup of the CIRFT has two rigid arms and linkages connecting to a universal testing machine. The curvature SNF rod bending is obtained through a three-point deflection measurement method. Three linear variable differential transformers (LVDTs) are clamped to the side connecting plates of the U-frame and used to capture deformation of the rod. The second portion of this report provides the latest CIRFT data, including data for the hydride reorientation test. The variations in fatigue life are provided in terms of moment, equivalent stress, curvature, and equivalent strain for the tested SNFs. The equivalent stress plot collapsed the data points from all of the SNF samples into a single zone. A detailed examination revealed that, at the same stress level, fatigue lives display a descending order as follows: H. B. Robinson Nuclear Power Station (HBR), LMK, and mixed uranium-plutonium oxide (MOX). Just looking at the strain, LMK fuel has a slightly longer fatigue life than HBR fuel, but the difference is subtle. The third portion of this report provides finite element analysis (FEA) dynamic deformation simulation of SNF assemblies . In a horizontal layout under NCT, the fuel assembly’s skeleton, which is formed by guide tubes and spacer grids, is the primary load bearing apparatus carrying and transferring vibration loads within an SNF assembly. These vibration loads include interaction forces between the SNF assembly and the canister basket walls. Therefore, the integrity of the guide tubes and spacer grids critically affects the vibration intensity of the fuel assembly during transport and must be considered when developing the multipurpose purpose canister (MPC) design for safe SNF transport.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2017

Characterization of Morphology using MAMA Software

The MAMA (Morphological Analysis for Material Attribution) software was developed at the Los Alamos National Laboratory funded through the National Technical Nuclear Forensics Center in the Department of Homeland Security. The software allows images to be analysed and quantified. The largest project I worked on was to quantify images of plutonium oxides and ammonium diuranates prepared by the group with the software and provide analyses on the particles of each sample. Images were quantified through MAMA, with a color analysis, a lexicon description and powder x-ray diffraction. Through this we were able to visually see a difference between some of the syntheses. An additional project was to revise the manual for MAMA to help streamline training and provide useful tips to users to more quickly become acclimated to using the software. The third project investigated expanding the scope of MAMA and finding a statistically relevant baseline for the particulates through the analysis of maps in the software and using known measurements to compare the error associated with the software. During this internship, I worked on several different projects dealing with the MAMA software. The revision of the usermanual for the MAMA software was the first project I was able to work and collaborate on. I first learned how to use the software by getting instruction from a skilled user at the laboratory, Dan Schwartz, and by using the existing user manual and examples. After becoming accustomed to the program, I started to go over the manual to correct and change items that were not as useful or descriptive as they could have been. I also added in tips that I learned as I explored the software. The updated manual was also worked on by several others who have been developing the program. The goal of these revisions was to ensure the most concise and simple directions to the software were available to future users. By incorporating tricks and shortcuts that I discovered and picked up from watching other users into the user guide, I believe that anyone who utilizes the software will be able to quickly understand the best way to analyze their image and use the tools the program offers to achieve useful results.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2017

Surveillance and Monitoring Program Full-Scale Experiments to Evaluate the Potential for Corrosion in 3013 Containers

A set of six long-term, full-scale experiments were initiated to determine the type and extent of corrosion that occurs in 3013 containers packaged with chloride-bearing plutonium oxide materials. The materials were exposed to a high relative humidity environment representative of actual packaging conditions for the materials in storage. The materials were sealed in instrumented, inner 3013 containers with corrosion specimens designed to test the corrosiveness of the environment inside the containers under various conditions. This report focuses on initial loading conditions that are used to establish a baseline to show how the conditions change throughout the storage lifetime of the containers.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Initial Development of a Method to Measure Carbon by Thermogravimetric Analysis-Mass Spectrometry

During HB-Line flowsheet development efforts at the Savannah River National Laboratory (SRNL), plutonium oxide (PuO 2 ) samples were produced using different precipitation and calcination conditions. To evaluate a potential cost savings for future analyses, this study measured the carbon (C) content of ten SRNL PuO 2 samples by two different methods: the accepted method of a carbon/sulfur (C/S) analyzer and a potential method of thermogravimetric analysis-mass spectrometry (TGA-MS). Though PuO 2 produced by HB-Line was not used in this study, the AFS-2 PuO 2 campaign is currently using TGA-MS for moisture analysis. Thus, using the same TGA-MS analysis for C could potentially provide a cost savings.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

ARIES team achieves major milestone in support of nonproliferation

The Advanced Recovery and Integrated Extraction System (ARIES) Program is a great example of LANL’s Weapons and Global Security programs working together to achieve important nuclear security mission goals. Executed at PF-4, a facility better known for its pit production mission, the ARIES Program is helping the nation meet its nonproliferation commitments by preparing surplus weapons-grade plutonium for final disposition. ARIES recently met a major milestone of producing 1 metric ton of plutonium oxide from material removed from surplus pits. The milestone was celebrated in an awards ceremony at LANL on January 28.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2020

Reactivity of a Cube, Cylinder, and Sphere

A water-reflected cube of dry plutonium oxide is found to be more reactive than a sphere of the same mass and composition. MCNP6 ® criticality results for a cube, sphere, and cylinder of identical density, mass, and volume are discussed in the context of several hydrogenous reflectors. Similar geometric comparisons are made for a fast metal system based on 240 Pu Jezebel.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2021

Evaluations of the Fates of Alkali Metals, Actinides, Mercury, and Iodine During DWPF Recycle Diversion

The fates of alkali metals, actinides, mercury, and iodine in the Defense Waste Processing Facility Recycle Diversion process (as currently conceptualized) have been evaluated through paper studies based on available knowledge of the chemistry, physical properties, solubility, and volatility of the various species involved. The effect of pH in the range from 9 to 13 has been discussed. Recommendations for additional studies to close technology gaps have been provided, many of which are contingent upon the results of pending testing and sample characterization efforts. There is uncertainty in the amounts of soluble actinides passing through the process filter, though the bulk of the actinides should be captured on the filter with the Recycle Collection Tank solids and the total amounts of actinides should be relatively low. The Recycle Collection Tank pH could impact the fraction of actinides reaching the evaporator, but the primary factors determining the actinide fate are expected to be the amount of CO 2 sorption from air sparging or, for certain actinides (such as plutonium), oxidation and/or sorption to MnO 2 solids from permanganate additions to destroy the glycolate anion. Process optimization could minimize the amounts of actinides passing the filter. Depending upon the levels of mercury observed in recycle stream samples and because of the volatility of mercury, the evaporator should be designed with the capability to remove dense mercury phases from the condensate to avoid exceeding ETP WAC limits. The facility design must be adequate to transfer dense mercury phases and testing to confirm mercury transfer is needed. Simulant containing mercury is recommended for both filtration and evaporation testing. OLI Modeling of the various recycle streams is recommended to provide insight on the fate of iodine. Iodine-spiked simulants are recommended for upcoming evaporation tests. The pro) ect should consider the likelihood and impact of NAS scale formation in the evaporators. Process optimization may be needed to minimize the accumulation of NAS scale and possibly the sorption of actinides in the evaporator. Actual waste testing of the Recycle Diversion filtration and evaporation should include the analysis of actinides, mercury, and iodine to determine their partitioning.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Prompt Gamma Analysis of ARIES Materials and Updates to the 2015 Calibration Equations

Prompt gamma (PG) analysis is a nondestructive, nuclear, elemental analysis technique that uses charged particle reactions to interrogate a sample, and elements present in the sample matrix are identified through the characteristic gamma-rays emitted from the product nuclei in alpha-p and alpha-n nuclear reactions. This technique has been applied to plutonium oxide packaged in over 4,000 individual 3013 containers, and the concentrations of certain light elements were determined from the integrated peak areas based on a calibration that was published previously. This report provides the results for a new population of 3013 containers packaged with oxide materials produced by the conversion of metal by Advanced Recovery and Integrated Extraction System (ARIES) project using the direct metal oxidation (DMO) process and muffle furnaces. New PG and analytical chemistry data collected since 2015 were added to the existing calibration data sets to refine the calibration parameters. Calibration equations were also developed for determining beryllium and fluorine at low concentrations in high-purity ARIES product oxides. The new fluorine calibration provides an order of magnitude greater sensitivity and results in an additional 1,408 containers in the original population identified as having fluorine as an impurity. Additionally, equations for calculating the lower limits of detection (LLDs) as a function of the actual counting time (live time) were obtained using WLS regression technique for samples in the calibration data set. This resulted in changes to the LLDs published previously.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Parametric Analysis of Holdup in HEPA Filters

This technical document (TECH) contains an analysis of several conditions deemed credible for plutonium oxide buildup in high-efficiency air particulate (HEPA) filters to determine the effect of holdup inside the filter on reactivity. This document is performed in accordance with NCS-AP-005, R3 [Ref. (1)].

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2013

Expanded Content Envelope For The Model 9977 Packaging

An Addendum was written to the Model 9977 Safety Analysis Report for Packaging adding a new content consisting of DOE-STD-3013 stabilized plutonium dioxide materials to the authorized Model 9977 contents. The new Plutonium Oxide Content (PuO{sub 2}) Envelope will support the Department of Energy shipment of materials between Los Alamos National Laboratory and Savannah River Site facilities. The new content extended the current content envelope boundaries for radioactive material mass and for decay heat load and required a revision to the 9977 Certificate of Compliance prior to shipment. The Addendum documented how the new contents/configurations do not compromise the safety basis presented in the 9977 SARP Revision 2. The changes from the certified package baseline and the changes to the package required to safely transport this material is discussed.

42 ENGINEERING↗

DOE OSTI2023

3D Source Reconstruction Using Coded Aperture Gamma-Ray Imaging

Recent measurements with coded-aperture imagers demonstrate material mass determination in a holdup setting to an accuracy within a few percent. This capability is of particular interest to the Surplus Plutonium Disposition (SPD) project, which aims to dilute and dispose of surplus plutonium oxide. Gamma-ray imagers can be used to determine holdup without interrupting normal operations. In this work, we examine techniques for 3D source localization and mass determination using gamma-ray imagers. Coded-aperture imagers provide excellent source localization within the 2D image plane; however, multiple imagers operating in tandem are necessary to identify source location in 3D space. A Maximum Likelihood Expectation-Maximization (MLEM) method for fitting detector mappings is a powerful tool for accomplishing this task. MLEM allows 3D source localization to be simultaneously constrained using multiple gamma-ray imagers by constructing the basis for the MLEM fit using detector mappings from different detector locations stitched together. Each of these basis points represents a singular response from a source in 3D space and is generated using Monte Carlo simulations of sources placed individually at different locations throughout the imager’s field of view. Additionally, implementing knowledge of the physical equipment in the simulations of the glovebox used for the SPD project incorporates attenuation effects that are needed to calculate material holdup.

Laminack, Alex↗

DOE OSTI2024

Progress Toward Gamma-Ray Imaging for Automated Holdup Measurement in Gloveboxes

Shielded gloveboxes are currently being constructed to facilitate dilution and disposal of many tons of excess plutonium oxide. Measuring holdup in these gloveboxes is expected to be challenging because of the limited available lines of sight through the glovebox shielding. A system of gamma-ray imagers is being developed to provide localization and quantification for holdup. The system will be mounted above the glovebox, where there is minimal shielding. Multiple imagers with overlapping coded-aperture fields of view are employed to enable three-dimensional reconstruction. Compton reconstruction is also available to localize sources outside the coded-aperture field of view. Improved uncertainties with respect to current techniques are expected by virtue of the fixed installation, spectroscopic performance of the detectors, and iterative image reconstruction techniques. Measurement campaigns have been undertaken at an active glovebox at Savannah River Site to test the gamma-ray imaging system in an operational environment, providing a simple test of a single imager that mimics the geometry of the installation proposed for future shielded gloveboxes. Data taken during quiescent periods in the glovebox were used to measure the buildup of material on an outlet filter and record a trend over time. Calibration data was taken with known sources to simplify analysis and provide a reliable assay of the filter. Resulting images make it possible to isolate the filter from other sources and recognize compromised data. This paper will present details of the measurement and analysis methods.

Schmitt, Kyle↗